Soil pH regulates the capacity of soils to store and supply nutrients, and thus contributes substantially to controlling productivity in terrestrial ecosystems 1 . However, soil pH is not an independent regulator of soil fertility-rather, it is ultimately controlled by environmental forcing. In particular, small changes in water balance cause a steep transition from alkaline to acid soils across natural climate gradients 2,3 . Although the processes governing this threshold in soil pH are well understood, the threshold has not been quantified at the global scale, where the influence of climate may be confounded by the effects of topography and mineralogy. Here we evaluate the global relationship between water balance and soil pH by extracting a spatially random sample (n = 20,000) from an extensive compilation of 60,291 soil pH measurements. We show that there is an abrupt transition from alkaline to acid soil pH that occurs at the point where mean annual precipitation begins to exceed mean annual potential evapotranspiration. We evaluate deviations from this global pattern, showing that they may result from seasonality, climate history, erosion and mineralogy. These results demonstrate that climate creates a nonlinear pattern in soil solution chemistry at the global scale; they also reveal conditions under which soils maintain pH out of equilibrium with modern climate.Climate controls many aspects of soil chemistry, affecting soil pH (ref. 4). Alkaline soils are known to be common in arid climates, while acid soils are known to be common in humid climates 1 . Surprisingly, however, the global-scale mechanisms governing this pattern remain broadly defined, and untested by direct observation. What are the dominant chemical equilibria that constrain soil pH? What aspect of climate defines the transition between alkaline and acid soils, and is the transition linear? The answers to these questions are fundamental to understanding soil development and surface geochemistry at the global scale. Furthermore, achieving this understanding may prove essential for representing soils in models of the terrestrial biosphere, given that soil pH controls many aspects of soil fertility 5,6 . Here we illustrate that simple geochemical and hydrological concepts can be used to build a mechanistic understanding of soil pH at the global scale.Interpretations of acid-titration experiments indicate that the soil pH is typically most strongly buffered by equilibrium with two secondary minerals: calcite (CaCO 3 ), or gibbsite (Al(OH) 3 ) 7,8 Fig. 1).Local studies of climate gradients have shown that the relative importance of these two buffers is determined by leaching, which removes Ca 2+ from the soil 2,3,8,9 . In climates where evaporative demand exceeds precipitation, leaching rates are low, and dissolved Ca 2+ accumulates as CaCO 3 -buffering soil pH near 8.2 (ref. 4). Conversely, in climates where precipitation exceeds evaporative demand, water leaches through the soil, removing Ca 2+ and allowing accumulation of relatively immobile...

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Soil moisture controls microbial activity and soil carbon cycling. Because microbial activity decreases as soils dry, decomposition of soil organic matter (SOM) is thought to decrease with increasing drought length. Yet, microbial biomass and a pool of water-extractable organic carbon (WEOC) can increase as soils dry, perhaps implying microbes may continue to break down SOM even if drought stressed. Here, we test the hypothesis that WEOC increases as soils dry because exoenzymes continue to break down litter, while their products accumulate because they cannot diffuse to microbes. To test this hypothesis, we manipulated field plots by cutting off litter inputs and by irrigating and excluding precipitation inputs to extend or shorten the length of the dry season. We expected that the longer the soils would remain dry, the more WEOC would accumulate in the presence of litter, whereas shortening the length of the dry season, or cutting off litter inputs, would reduce WEOC accumulation. Lastly, we incubated grass roots in the laboratory and measured the concentration of reducing sugars and potential hydrolytic enzyme activities, strictly to understand the mechanisms whereby exoenzymes break down litter over the dry season. As expected, extending dry season length increased WEOC concentrations by 30% above the 108 μg C/g measured in untreated plots, whereas keeping soils moist prevented WEOC from accumulating. Contrary to our hypothesis, excluding plant litter inputs actually increased WEOC concentrations by 40% above the 105 μg C/g measured in plots with plants. Reducing sugars did not accumulate in dry senesced roots in our laboratory incubation. Potential rates of reducing sugar production by hydrolytic enzymes ranged from 0.7 to 10 μmol·g ·h and far exceeded the rates of reducing sugar accumulation (~0.001 μmol·g ·h ). Our observations do not support the hypothesis that exoenzymes continue to break down litter to produce WEOC in dry soils. Instead, we develop the argument that physical processes are more likely to govern short-term WEOC dynamics via slaking of microaggregates that stabilize SOM and through WEOC redistribution when soils wet up, as well as through less understood effects of drought on the soil mineral matrix.

The problem of reducing the impacts of rising anthropogenic greenhouse gas on warming temperatures has led to the proposal of using stratospheric aerosols to reflect some of the incoming solar radiation back to space. The deliberate injection of sulfur into the stratosphere to form stratospheric sulfate aerosols, emulating volcanoes, will result in sulfate deposition to the surface. We consider here an extreme sulfate geoengineering scenario necessary to maintain temperatures at 2020 levels while greenhouse gas emissions continue to grow unabated. We show that the amount of stratospheric sulfate needed could be globally balanced by the predicted decrease in tropospheric anthropogenic SO2 emissions, but the spatial distribution would move from industrialized regions to pristine areas. We show how these changes would affect ecosystems differently depending on present day observations of soil pH, which we use to infer the potential for acid-induced aluminum toxicity across the planet.